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在现场电化学重建铜单站到双站的环境尿素合成

Jiafang Liu^1,2, Shengbo Zhang^1,2, Zhixian Mao^1,2

¹Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei, 230031, China.

Angewandte Chemie (International ed. in English)

|July 30, 2025

概括

研究人员开发了一种铜单原子催化剂 (Cu-N3 SAs),该催化剂通过CO2和NO3-电还原转化为双原子位点,以有效地合成尿素.

科学领域:

电触媒溶解是一种电触媒.
材料科学材料科学材料科学
可持续化学可持续化学

背景情况:

高效的尿素合成对农业和工业至关重要.
识别催化活性位点是优化碳联反应的关键.
电化学减少CO2和NO3-提供了可持续的生产尿素的途径.

研究的目的:

设计和研究一种新的铜单原子催化剂 (Cu-N3 SAs) 用于电化学尿素合成.
为了阐明反应期间的结构演变和活性位点动态.
要了解二氧化碳和NO3 - - 减少为尿素的机制.

主要方法:

铜单原子催化剂与Cu-N3协调的合成.
在现场X射线吸收光谱 (XAS) 探测结构变化.
在现场光谱学与质谱学相结合,以确定反应中间体.
电化学测量以评估尿素合成性能.

主要成果:

Cu-N3 SAs经过电化学重建,形成N2-Cu-Cu-N2双站点.
这些双站点表现出增强的尿素合成性能.
反应机制涉及*CO和*NH中间体,在双位点形成*CONH.
双站点可促进二氧化碳吸附和多电子转移,从而降低能量屏障.

结论:

从单原子部位到双原子部位的电催化结构重建是增强尿素合成的有效策略.
N2-Cu-Cu-N2双位点是二氧化碳和NO3-到尿素的电化学联合减少的关键活性位点.
这项工作为有效的尿素电合成提供了对活性部位动态和反应机制的基本见解.

关键词:

一个 Cu 单个原子.电催化尿素合成电催化尿素的合成.在现场进行重建.结构性的可逆性结构性的可逆性

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